Results in Engineering 15 (2022) 100474

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Results in Engineering
journal homepage: www.sciencedirect.com/journal/results-in-engineering

Band gap formation of 2D materialin graphene: Future prospect

and challenges
Rajib Nandee a, Mohammad Asaduzzaman Chowdhury a, Abdus Shahid b, Nayem Hossain c, *,
Masud Rana a
a
Department of Mechanical Engineering, Dhaka University of Engineering and Technology (DUET), Gazipur, Gazipur, 1707, Bangladesh
b
Department of Textile Engineering, Dhaka University of Engineering and Technology, Gazipur, Gazipur, 1707, Bangladesh
c
Department of Mechanical Engineering, IUBAT-International University of Business Agriculture and Technology, Bangladesh

A R T I C L E I N F O A B S T R A C T

Keywords: Graphene, a single particle thicker carbon layer with a hexagonal form, was successfully confined, and the po­
Graphene tential electrical impact was observed in 2004. Since a surge in study interest has risen, concentrating on its one-
Bandgap of-a-kind semimetallic property ascribing to the intersection of the π and π* groups at the Fermi level at K and K′
Sizeable band gap
focuses in reciprocal space. At energies around the decadence point, these bands are also directly dispersive,
Tunable band gap
resulting in zero-mass quasiparticles (Diracfermions) linked to the equivalence of the two sublattices in the
Electron
Silicon primitive unit cell of graphene. The electron’s relativistic nature makes optimal transmission across high po­
Semiconductor tential barriers possible (Klein paradox). As a response, graphene is frequently predicted to be the structural
obstruct for future electrical devices. Future semiconductor industries could replace silicon because of its unique
electrical and transport capabilities, but it lacks liveliness. For practical applications, the bandgap is a generous
limitation. From the earliest starting point, it can be said that halting symmetry may be the most productive
methodology to recognize bandgap tenability in graphene. As indicated by uniaxial or in-plane shear strain, the
weak cross-section twisting of graphene has led some to believe that most stressed graphene has lost energy
below 1eV. The limitations of the present work as well as future research directions were also discussed here.
Theoretically, a sizeable band gap of ≥2 eV, tunable bandgap with the desired level, and low contact resistance in
metal interfaces are still being explored. Nonetheless, they are less understood. Future studies can be carried out
experimentally to resolve the constraints of semiconductors for their applications in a variety of fields.

Credit author statement
Rajib Nandee and Mohammad Asaduzzaman Chowdhury: Concep­
tualization and writing, Md. Abdus Shahid and Nayem Hossain: Writing
and editing, Md. Masud Rana: Review & Editing.
1. Introduction
Semiconductor graphene virtually contains a unique property having
the bandgap practically zero. Additionally, charge carrier velocity in
graphene and at the conduction band’s base does not reduce as it does in
other materials at the beginning of the valence band, but remains con­
stant throughout the whole spectrum, especially where the conduction
and valence bands meet at the Dirac point (Fig. 1). Switching between
states with low conductivity the input voltage can change the thickness
of the states in graphene. Insulators (diamond), semimetals (graphite),
qubit/bit (fullerenes), and 1D semiconductors or metals, graphene, and
carbon nanotubes are all made from carbon. Graphene particles are
organized in a honeycomb-like 2D cross-section. Stacked graphene
layers can be used in a sp2 hybridized structure to synthesize carbon
nanotubes, fullerenes, and graphite. Since graphene has a stronger
carbon-carbon bond than diamond, it is extremely stable and chemically
inert. Low graphene life structure decanter exhibits a conduction and
valence band corresponding to the charge-neutral level. A typical
semiconductor has a bandgap of 1–2 eV, but graphene has none, making
it an exception. Furthermore, single-layer graphene possesses direct
electron energy force capacitance, and it corresponds to all other semi-
two-dimensional materials with an amount of energy. Graphene has

* Corresponding author.
E-mail addresses: r.nandee@gmail.com (R. Nandee), asad@duet.ac.bd, asadzmn2014@yahoo.com (M.A. Chowdhury), te_shahid@yahoo.com, shahid@duet.ac.bd
(A. Shahid), nayem.hossain@iubat.edu (N. Hossain), mrdeeptoduet@gmail.com (M. Rana).

https://doi.org/10.1016/j.rineng.2022.100474
Received 9 May 2022; Received in revised form 24 May 2022; Accepted 26 May 2022
Available online 25 June 2022
2590-1230/© 2022 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
R. Nandee et al. Results in Engineering 15 (2022) 100474

Fig. 1. The energy dispersion variation of graphene lattice [3].

similarities with photons in connection with linear energy-momentum

scattering the relativistic Dirac condition describes free space. This in­
dicates that all electrons are free of their energy, move at a constant
speed, and act as if they have no mass. At the Dirac point, this is true also
when the thickness of the states evaporates. The superior electrical
Fig. 2. Geometric structures of Si-substituted graphene systems for (a) 100%%
structure of graphene, for example, has had a significant impact on the
Si substitution, (b) 50%% Si ortho-/para-substitution and (c) 50%% Si meta-
new integer quantum Hall impact [1,2], observed in this remarkable substitution [91].
material.
On the other hand, graphene is a one-particle-thick 2D material
unmatched mechanical power. Despite the fact that a limited bandgap is
made of carbon atoms embedded in a honeycomb mesh. Extensive
a key characteristic of numerous electronic and optical systems, gra­
investigation into every aspect of this new substance is being sparked by
phene’s lack of a power bandgap hinders the development of elite
ongoing scientific discoveries [4,5]. The Brillouin zone’s conductivity
field-impact transistors (FET) and optoelectronic devices [31,46–53].
and valence groups meet at six Dirac points, according to graphene’s
Furthermore, it is particularly difficult to control the Fermi level of
tight-binding calculations [1], where energy dissipation occurs by en­
graphene across a wide range in order to avoid heterojunction energy
ergy. This remarkable band scattering in graphene shows new electronic
barriers, consequently limiting the advancement of graphene-based
and physical properties, including the quantum Hall effect at room
electrical and optoelectronic products. Although outward methods
temperature and the high portability of the charge carrier [1,6,7]. It
[49,50] and hydrogen adsorption [51] have been used to open the
cannot be used for nano-electronic applications as it is a gapless semi­
bandgap and regulate the work capacity of graphenes, such as doping
metal and has a pristine structure. That is why, opening a limited hole is
[52,53] and multilayers, they have until now failed to tune work and
important for different systems at the K point in the energy scattering [8,
consistently yielded massive bandgaps (consistently 1 eV). In conse­
9]. Graphene on BN substrates exhibits a small gap (100 meV) [10,11].
quence, gadgets based on graphene are still limited in terms of perfor­
Furthermore, for silicon carbide substrate, 250 meV band gaps are
mance [54]. In order to fully understand graphene’s potential in the
recognized [12,13]. An incredible effort is given to generate the gap
semiconductor industry, a new technique is needed for adjusting its
around 1 eV similar to germanium/silicon for use in computerized
electron energy structure. Graphene’s inherent inadequacy can be
gadgets. In SiC sub-lattice, carbon lamina is covalently bonded accord­
improved through strain-engineering by opening the bandgap. On the
ing to ongoing work [14–18]. Asymmetry breach in the system causes
basis of the lattice symmetry, the wave vector at K point in graphene. It
the bandgap for graphene to ruthenium metal to arise [19,20]. McCann
has been proposed that uniaxially applied tensile or compressive strain
and Falko [9,21] report that when a transverse electric field is produced
perpendicular or parallel to the C–C bonds will disrupt the lattice sym­
between two faces of the framework, a two-layer graphene gap is
metry and thus create a bandgap and adjust the work function. Despite
formed. Infrared spectroscopy [22,23] and edge settled photograph
this, most strain-engineering work has only yielded small bandgap
discharge spectroscopy (ARPES) [24] band gap in graphene with two
openings, without any control over nanoscale bandgaps. Bilayer gra­
layers (bi-layer) [24]. Using attractive collaboration altered by the use of
phene’s bandgap was previously opened to 0.3–0.4 eV using shear
phonons in a polarizable substrate to compute the bandgap in graphene
strain. A first-principles calculation by Gui et al. and Hicks et al. [55]
substrate, Hague [25,26] presented a model to compute the bandgap in
observed that simultaneous enlargements of C–C rings in two perpen­
graphene substrates. The bandgap can be set up in graphene having a
dicular axes could result in a pseudogap of 0.48 eV. Aziza et al. [56–58]
few requests in eV [27] and Fluorographene [28,29] by chemical
predicted that the pentagonal and heptagonal rings resulting from
alteration of the framework with hydrogen and fluorine, individually.
stacking faults and partial dislocations in graphene sheets would cause
Atomic thick boron nitride (BN) structures a honeycomb grid causes a
the opening of the 0.8 eV bandgap [59].
gap of 2δ where the p orbitals on N destinations pare moved up in energy
Stacking faults and partial dislocations associated with pentagonal
by +δ and diminished in the energy of - Δ [30]. A band hole of 5.56 eV is
and heptagonal rings of graphene would cause a 0.8 eV bandgap
being monitored cautiously in monolayer BN frameworks. A 2D atomic
opening suggested by a recent paper [60]. This resulted in a significant
layer of sp2 hybridized carbon, graphene is one of the most promising
bandgap opening of 0.8 eV. Furthermore, it has been reported that strain
materials for the future [1–3,31–45] because of its high electronic
and curvature simultaneously alter the energy band structure in gra­
versatility, quantum Hall impact, high thermal conductivity, adapt­
phene, potentially resulting in bandgaps greater than 1 eV [60–62].
ability, optical transparency, molecular anchoring ability, and

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R. Nandee et al. Results in Engineering 15 (2022) 100474

Fig. 3. Graphene synthesis techniques.

2. Process of band gap formation
2.1. Doping
As a method of balancing the characteristics of bulk materials,
doping of graphene is an appealing method for producing its band
structure [63–90]. It is normal to employ substituent atoms from the
periodic table’s second row. A thorough study of the electronic prop­
erties of graphene doped with B or maybe N has been conducted. A
variety of B/N-co-doped graphenes (Fig. 2), such as graphene doped
with BN, (BN)3, and (BN)12, are also quite exciting, along with B- or
N-doped graphene [67]. The doping setup, and bandgaps are nonlinear.
The outcome depends on the concentration of BN domains. Quantum
restrictions play a significant role in the establishment of a bandgap in
large regions of BN with high focuses. However, quantum confinement
factors alone cannot explain why BN with low concentrations can open a
large bandgap. There is little variance in the size of BN gaps in
low-concentration locations, indicating that the bandgap is adjusted
accordingly. The band structure of the ordered alloy (BN)x (C2)1 x has
also been studied. With a minor concavity, the bandgap value and
dopant concentration have a nearly linear relationship. The bandgap is
due to the interaction between graphene and BN Bloch states. The
nonzero bandgap in BN-doped graphene has also been studied theoret­
ically [71]taking into account alternative edge configurations (zigza­
g/armchair) as well as the symmetry of the superlattice containing BN
quantum dots (QDs). The bandgap is largely determined by the width of
the carbon wall between nearby BN QDs. A thermal synergist CVD
approach may be used for including large territories of h-BNC materials
[72]. Hybridized patches of BN and C phases are randomly scattered,
ranging from pure BN to pure graphene. Additionally, it has supple­
mentary highlights that are different from those found in graphene,
h-BN, or intermittent B/N-codoped graphene. The low-voltage deviation
amended high-goal transmission electron microscopy (HRTEM) can be
used to examine the atomic structure of a single layer. The figure shows
a rapid Fourier change (FFT) obtained from the image, which reveals a
hexagonal nuclear structure. It is common to see turbostratic stacking in
several layers, and the various Moire’ shapes seen in nuclear scale
photos are due to the absence of an AB stacking vault between layers. By
using UV–visible retention spectra, we determined optical bandgaps of
1.62 eV for samples with 65 atom percent C and 1.51 eV for samples
with 84 atom percent C. It was found that the h-BN regions and the
graphene spaces were sufficiently large to protect their respective
bandgap features and effectively form a superlattice, as shown by the
two distinct optical bandgap values. A violation of the inherent pro­
portionality of graphene sublattices is attributed to the widening of the
bandgap in graphene doped with BN. In graphene nanoribbons, an
increase in BN fixation results in a decrease in the bandgap due to the
construction of small graphene spaces bounded by large BN regions.
3. Synthesis of graphene
Many methods have been discovered to distribute slender graphitic
films. Since the late 1970s, it has been known that carbon accelerates as
tiny graphitic layers on advanced metal surfaces [92,93]. A diagram­
matic representation of the synthesis techniques of graphene is shown in
Fig. 3. However, due to the difficulty of isolating and transporting them
onto protective substrates, the electrical properties of these materials
have never been studied. Nonetheless, Ruoff and coworkers attempted
to segregate sparse graphitic particles on SiO2 substrates by the me­
chanical scouring of planned islands on HOPG in the late 1990s [94].
However, no information has been found on their electrical properties.
Kim and colleagues reported on electrical characteristics in 2005 [95].
The graphene gold rush began when Geim and colleagues isolated gra­
phene onto a SiO2 substrate and tested its electrical properties. After the
discovery of graphene in 2004, numerous methods have been developed
to produce narrow graphitic films with little or no layer of graphene. The
methods will be discussed in more detail further down.
3.1. Epitaxial growth on metals
Researchers have studied ultrathin graphitic coatings epitaxially
grown on metal surfaces for a long time [92,96–105]. Recently, epitaxial
single-layer graphene films have been made using the same metals
[106–114]. At high temperatures, most of these metals exhibit reactant
migration. There are three types of carbon isolation: carbon fume
deposition [110], carbon substance deposition [115], and hydrocarbon
degradation on the catalytic metal surface [116]. In each of these
findings, the development was carried out using UHV settings on
metallic single crystals. In an isolation-controlled growth under a high
vacuum, the metal single crystal is heated to high temperatures to
dissolve the interstitial carbon in the metal grid. Subsequent cooling of
the metal crystal causes the solvency to decrease dramatically, isolating
the carbon at the surface, which develops into graphene layers. K F
McCarty and colleagues studied the components, energy, and elements
of epitaxial graphene growth on metallic single precious crystals in
detail [116–118]. In their interpretation, the rate of graphene nucleation
and development is inextricably linked to the concentration of surface C
adatoms. However, the restricting factor in graphene development en­
ergy is a connection to the graphene islands rather than surface diffu­
sivity of C adatoms. They also indicate that growth pace is influenced by
direction. According to this property, graphene growth is fundamentally
determined by the arrangement of C atoms at the island’s borders and

3
R. Nandee et al.
Fig. 4. (a) Two routes for mechanical exfoliation; (b) Micromechanical cleavage for graphene production [134].
their connection to the substrate. Graphene nucleus and carbon molec­
ular cluster have a much better connection than the C monomer
connection provided by non-direct development energy. Graphene de­
velops through surface adatom dispersion rather than bulk diffusion.
The development rate is also unaffected by the presence of a C adatom
source. Researchers studied graphene development components using
time-resolved angle-resolved photoemission spectroscopy [119]. Due to
the discrepancy between the grids of the metallic substrate and gra­
phene, intermittent moires were observed on epitaxial graphene [106,
108,109,111,116,120,121].
A memoir superstructure on epitaxially produced monolayer
graphite has been explained as early as 1992 [116]. If a cross-section
discrepancy is above 1%, as it is with Ir, Ru, Pt, and Pd, these moires
are found in STM analyses regardless, however they are not visible if
epitaxial growth occurs on Ni [97,107] and Co [107,122]. Intermittent
disturbances or Moire edge confusion can also be eliminated by incor­
porating absorbed oxygen on the metal surface with graphene and the
metal surface [123]. In situ UHV chambers are most commonly used to
study epitaxial graphene layers on metallic single crystals. The most
common methods for characterizing materials are reflected high energy
electron diffraction (RHEED), low energy electron diffraction (LEED),
low energy electron microscopy (LEEM), and Auger electron spectros­
copy (AES). As part of several tests, AFM and STM investigations were
also carried out to investigate the Moire edges. LEED and LEEM (or
RHEED) are used to obtain images and diffraction patterns across the
substrate, allowing correlation between picture changes and graphene
formation. AES is commonly used to determine and plan C adatom
concentrations on a surface to obtain nucleation and development sys­
tems, which provide significant information as a function of time and
temperature. In addition to being prohibitively expensive and inflexible,
the process uses single crystal metallic substrates and high UHV tem­
peratures to grow. It is still a work in progress to transfer epitaxial
Fig. 5. (a,b) Top and side view of monolayer graphene. (c) The band structure of graphene along the high symmetry Γ− M − K − Γdirections and the associated
Brillouin zone. The zero in the energy axis is set at the Fermi level as shown by the solid line [158].
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Results in Engineering 15 (2022) 100474
graphene onto self-assuring substrates. Thus, with the existing state of
knowledge and understanding, commercialization of this development
process is not feasible.
3.2. Mechanical exfoliation
Since the 1970s, it is a known fact that as slim graphitic layers carbon
precipitates on transition metal surfaces [124,125] but until metallic
substrates are found there are no reports on their electronic properties
and no attempts on how to move them on protecting substrates. Ruoff
and co-workers tried mechanical rubbing of patterned to isolate thin
graphene flakes in the late ’90s on SiO2 on HOPG [126]. However, the
electrical property characterization report is absent from their work.
Kim and coworkers achieved this using a similar method in 2005 and
they reported electrical properties [127]. The main report on detaching
graphene has been prepared by Gein and colleagues who detached
graphene in 2004 by mechanical peeling onto a protective SiO2 substrate
[128]. From that point forward, various methods produced light
graphitic films and very little layer graphene from mass graphite or
HOPG. In order to obtain single-layer graphene flakes on desired sub­
strates, mechanical shedding may be the strangest and most well-known
technique. This strategy generates graphene drops from HOPG through
continuous stripping/shedding (Fig. 4). This stripping/peeling should be
possible with a variety of specialists such as scotch tape [128] ultra­
sonication [129] electric field [130] and even by transfer printing
strategy [131,132] etc. To improve single-chip formation, the HOPG is
bonded to the substrate using regular glue, such as epoxy gum [133] to
the substrate so that it can improve the formation of a single chip.
Transfer printing of plainly visible graphene designs from planned
HOPG using gold films is also shown in an ongoing report [133]. It is by
far the cheapest method of producing high-quality graphene. AFM,
Raman spectroscopy, and optical microscopy usually explain graphene
R. Nandee et al.
flakes achieved by mechanical shedding. Single-layer graphene can be
recognized through optical microscopy which is considered one of the
most famous strategies.
A trademark shading contrast can be found contingent upon the
thickness of graphene flakes on the head of Si wafers thermally devel­
oped SiO2 having 300 nm thickness [135] (Fig. 2). Raman spectroscopy
is additionally done on graphene gotten by mechanical peeling. It is the
speediest and most exact strategy for recognizing the thickness of gra­
phene chips and deciding their crystalline quality. This is on the grounds
that graphene shows trademark Raman spectra dependent on the
number of layers present [136–138]. The thickness and number of layers
of peeled graphene can be confirmed by AFM analysis. This technique
may find solitary layer flake acquiring single or few-layer graphene
which is actually poor. Exceptionally little graphene flakes are acquired
with dimensions of microns to a few millimeters. Hence this strategy is
practicable just on a research facility scale and isn’t versatile to a
commercial level.
3.3. Physical adsorption
Unlike chemical modification, the physical deposition of atoms onto
the interface of monolayer and bilayer graphene maintains the sp2
carbon atoms C–C interactions in the crystal arrangement. As a result,
charge redistribution, potential modulation, and the formation of a
Moire’ sequence can all be linked to physical adsorption opening a
bandgap [139–157]. In a study [139] that employed ARPES and STM to
study Na adsorption effects on the band structures of exposed graphene
and graphene grown epitaxially on Ir (111), an Ir cluster superlattice
was added to the exposed graphene. A sketch of graphene’s atomic
structure and its band dispersion, together with sketches of graphe­
ne/Na/Graphene/Ir and graphene/Ir/Na, can be found in Fig. 5,
respectively. The graphene layer shows up a huge bandgap of 740 meV
by adsorbing Na particles on the head and adsorbing onto an Ir group
superlattice. Two potential systems are proposed, to be specific, the
change of the crystal potential by Na adatoms and the commensurability
of the period of Na adatoms as for the Moire’s example of graphene on Ir.
Notwithstanding physical adsorption on monolayer graphene, adatoms
on bilayer graphene can likewise change the band structure of graphene.
Electronic states close to the Fermi level can be controlled by controlling
the bilayer graphene’s bearer thickness.
Additionally, BLG is doubly doped with FeCl3 acceptor and K donor,
resulting in a bandgap of 0.27 eV due to symmetry breaking and a _0.09
eV shift in the DP due to FeCl3’s strong electronegativity [141]. Some
other adatoms, such as Li [142,143] 3d transition metal atoms (e.g., Sc,
Ti, V, Mn, and Fe) noble metal atoms (e.g., Cu, Ag, and Au) [144], 5d
adatoms [145] water and other gas molecules (NH3, HF, CO, etc.) [154,
155] tetrafluorotetracyanoquinodimethane (F4-TCNQ) [148,149]
organic molecules [150] and so on have also been investigated for
bandgap engineering in graphene.
3.4. Carbide epitaxial growth
The development of epitaxial graphene on metal carbides has been
studied for several years [159–166]. No reports show the use of silicon
carbide as an epitaxial development substrate. Because previous use was
based on nature, detailed research on the electrical properties of
monolayer graphene has not been done. However, the first report on
electrical studies based on epitaxial graphene developed on SiC
appeared in 2004 [167]. Because SiC is a semiconductor with a wide
bandgap of 3 eV, it is able to perform electrical estimation to use this
substrate. The development of epitaxial graphene on SiC requires UHV
conditions, which is costly. Epitaxislly graphene in SiC poses numerous
challenges. Furthermore, the gadget level is not up to par. To break
through this barrier, researchers created epitaxial graphene with 900
bar barometrical weights in an argon climate. Graphene film developed
in the argon region [168]. Also, it demonstrates high carrier mobility,
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Results in Engineering 15 (2022) 100474
crystalline quality, and Hall conductivity. The systems and energy of
epitaxial graphene development on SiC have also been revealed in a few
studies [169,170]. Fig. 1 represents a schematic of the synthesis pro­
cedure. According to literature, vacuum graphitization can improve the
produced nature of films. Temperatures can also be reduced by intro­
ducing a small amount of Si vapor pressure by means of disilane. This
activated the development of large-area graphene chips with uniform
thickness while also reducing the warm etch pit arrangement. HRTEM
analysis shows that increasing graphitization temperature improves
graphene temperature, which nucleates along the 1–10 n planes on the
SiC surface [171]. On the hexagonal face of 6-H SiC, similar HRTEM
analyses have been performed [171]. Epitaxial progression on SiC has
also been accomplished without the use of Si sublimation. This is
completed by a further supply of carbon. This extra carbon is provided
by Molecular Beam Epitaxy, which includes the sublimation of solid
carbon or hydrocarbon gas decay [172]. Effective arrangement of a
graphene monolayer on NbC, TaC, HfC, ZrC, and TiC surfaces by
ethylene disintegration several years ago [160,161]. MBE can perform
epitaxial development on SiC at moderately low temperatures. Another
study [173] looked into epitaxial graphene grown on SiC by evaporating
split ethanol at 950 ◦ C. These strategies, which include additional car­
bon dissipation, prevent remaking of the SiC surface, which occurs
during warm graphitization due to higher temperatures and results in
lopsided and harsh surfaces. This wonder can likewise be forestalled by
utilizing these strategies. STM and AFM analyses, and LEEM, LEED,
RHEED, HREELS, and ARPES, epitaxially developed graphene on car­
bides. The use of the vast majority of these methods has been depicted
previously. HREELS is also used to study phonon scattering curves in
epitaxial graphene [174]. This aids in comprehending how developed
graphene interacts with the substrate. Epitaxial graphene development
on SiC has improved techniques for graphene production and commer­
cialization for applications in electronics. Because SiC is a wideband
hole semiconductor, gadgets can be created without transferring. This
makes gadget manufacturing entirely achievable and practical. Be that
as it may, there are as yet numerous deterrents to defeat such an
acknowledgment. According to the union, a specific test is an enormous
territory of single-layer graphene development on the wafer-scale sub­
strate. Another test is the advancement in the nature of graphene as a
result of this strategy.
3.5. Wet chemical synthesis
Chemical techniques that produce graphite and graphite intercala­
tion compounds as by-products can produce both colloidal suspensions
of graphene and chemically modified graphene, making graphite
another excellent source for graphene synthesis. Graphene and chemi­
cally modified graphene have many applications, including paper-like
materials [175–180] polymer composites [181] energy storage mate­
rials, and transparent conductive anodes. Graphite oxide was first
created in 1860, and since then, it has largely been produced by Brodie,
Hummers, and Staudenmaier strategies. Oxidation of graphite is
included among these strategies in presence of solid acids and oxidants.
Graphite oxide has a hydrophilic layered structure of graphene oxide
sheets. As a result, it is usefully intercalated with water. A strong
state-marked NMR has been applied to examine graphite oxide which
has illuminated its structure. Further understanding of graphite oxide
about its nuclear structure using NMR investigation has been demon­
strated by another article [182]. Breaking graphite oxide with sonicat­
ion or blending will yield graphene oxide. The arrangement of this
colloidal suspension can be done using natural solvents or in water. This
colloidal suspension of graphene oxide can be reduced by various
techniques to frame the suspension graphene sheets depicted in (Fig. 1)
when the dried dark powder is found. However, because it contains
some oxygen, perfect graphene oxide cannot yet be obtained. Homo­
geneous colloidal suspensions of CMGs functionalized have been
accounted for in a variety of solvents, with various gatherings. In a few
R. Nandee et al.
Fig. 6. Growth mechanism of graphene on the metal substrate [190].
studies, CMGs have been functionalized with gold or TiO2, and colloidal
scatterings of graphene and CMGs have also been demonstrated using
graphite or graphite intercalation compounds [182] or expandable
graphites. A homogeneous colloidal suspension of graphene sheets or
strips can be found by mixing N-methyl pyrrolidone (NMP) with
potassium-based graphite intercalation compound (K (THF)x C24).
Polymer-covered graphene scatterings in natural solvents have also been
synthesized successfully. Such scatterings have been basically integrated
from expandable graphite. A fluid suspension of graphene has been
discovered in expandable graphite and has been accounted for. This
method produces graphene sheets with organic molecular coatings.
Electrochemical treatment of commercial graphite poles results in ionic
fluid functionalized graphene in a stage isolated blend of water and ionic
fluid [183]. CMGs and colloidal graphene suspensions are excellent
candidates for the preparation of paper-like materials, transparent
conducting films, and graphene bases composite. Colloidal graphene has
now been legitimately shed, thanks to careful solvent selection and
sonication. It was then separated into different portions based on layer
thickness using Density Gradient Ultracentrifugation. It will likewise
end up being promising for sensor applications [184]. These are not
suitable for some electronic applications as they contain impurities and
have high deformity thickness. Colloidal stability and scalability are a
growing concern. Finally, for additional improvements to inappropriate
paths, a much better and more careful response mechanism, and struc­
ture are required. Finally, for additional improvements to inappropriate
paths, a much better and more careful response mechanism, and struc­
ture are required. For a point-by-point analysis aimed at chemically
derived graphene and CMGs, see Ref. [185] by Park and Ruoff.
3.6. Chemical vapor deposition
Epitaxial development on metallic single crystal and epitaxial
development on metallic thin film are fundamentally the same. CVD
deposition, on either hand, needs more pressure than monolayer pro­
gression, and the metallic bases form in the form of films or foil during
the process. Here, the substrates are found to be polycrystalline in nature
as these are thin films or foils. Besides, the individual crystals or grains
are found to be situated arbitrarily. On graphene film, carbon regions
with higher thickness after isolation happen. Copper and nickel sub­
strates are mostly used for graphene development by a CVD method. It’s
exciting to note that each of these elements has its own scheme. The
primary substrate on which CVD growth of large-area graph was
considered was a nickel. These efforts have begun as soon as 2007 [186].
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Results in Engineering 15 (2022) 100474
However, stronger governance of the methodology was not attained,
and as a result, the work went mostly ignored. Around late 2016, the
first credible claims of a census of large-area diamonds on nickel sur­
faces arose in 2008 and mid-2009. These results generated a resurgence
of interest in diamond CVD amalgamation. After then, a slew of studies
looked into modules and how to strengthen preliminary study and
criteria. Nickel substrate has a significant negative perspective as the
development procedure isn’t self-restricting. Another negative
perspective is the formation of countless folds and wrinkles on the films.
Wrinkles or folds in the material are induced by either a variation in
nickel and graphene heat transfer or deformity nucleation at step edges
on the Ni layer. The proposed site structure is similar to epitaxy on Ni
single crystals. In CVD development each grain goes about as a solitary
crystal. Better graphene development can be found along with Ni (111)
surface as the grid mismatch is least with Ni (111) surface. By creating a
finished Ni film, the nature of graphene films along these lines can be
altogether improved and can be performed by a specific annealing
treatment. Additional studies on cooling rates of graphene thickness and
quality have been performed [187]. According to the study, carbon gets
stuck inside the nickel lattice, and low cooling rates create thick graphite
films, but higher flow rates (100 C/s) do not result in any formation. A
crystallinity of 10–15 ◦ C/s has been shown to be ideal for the growth of
1–2-layer films. Ongoing research on CVD development indicates copper
to be a more encouraging substrate [188]. This is due to fact that dia­
mond production on copper is inner, meaning it ceases after one layer.
Furthermore, copper foils can be utilized to create top-notch films that
contain most part of the SLG. The system for graphene development on
copper is unique in relation to that of nickel. The primary reason for this
is the great difference in charcoal’s strong solvency of both copper and
nickel. Limited solvency and strong dissolvability of carbon are seen in
copper and nickel respectively. The copper substrate cannot diffuse
carbon that much as well. A schematic view of the development process
is shown in Fig. 6. The carbon atom, as well as the vapor pressure of the
carbon source, determines the development of copper surface occur­
rences to a great extent. However, one weakness is the synthesis of
top-notch single-layer graphene film with copper substrate requires CVD
development. For this 500 mtorr low pressure are basic to obtain great
films. No distinction is observed in crystalline quality from graphene
developed on copper foils that need the least surface readiness along
these lines. Advancement in boundary development has been achieved
by using methane by graphene incorporated with the crystalline nature
of CVD. Studies show that gaseous precursor at surrounding pressures
and high methane fractional pressure is utilized to develop multilayer
R. Nandee et al.
films. The Ruoff group has developed large space area constancy of
nanosheets with exceptionally high mobility values in the scope of 12,
000–16000 V cm− 1. Utilization of high temperature as well as low
methane incomplete strain is the two-stage process that can power low
thickness cores arrangement which has been trailed for quick as well as
ceaseless single layer development by high-temperature high methane
fractional weight. A similar gathering has been utilized to show a similar
process with high-temperature carbon single crystals up to 0.5 mm
across grown up on copper foils at temperatures exceeding 1035 ◦ C.
Srivastava’s fluid antecedent integrated proper quality with respect to
large regions to produce another ongoing success in CVD graphene
pairing [189]. In this work huge territory of great graphene, the com­
bination has been done utilizing fluid antecedent hexane. A huge
centimeter size graphene film on Si/SiO2 substrate can be seen in Fig. 3.
Utilizing a fluid precursor presents numerous points of interest over
conventional vaporous antecedents and diminishes the severity of trial
conditions. Boron and nitrogen can have advancement in substantial
synthetically doping to graphene because boron and nitrogen contain
natural fluids that can be accessed efficiently and effectively as a liquid
precursor can be handled easily. At the point when it was demonstrated
that CVD development should be possible utilizing vaporous and liquid
precursors, strong antecedents shouldn’t be abandoned.
Tour and his collaborates finished this puzzle by proficiently syn­
thesizing a huge area of graphene using strong carbon antecedents on
copper foils. The researcher spin-coated the 100 nm film on copper foils
followed by annealing these coated foils maintaining the temperature of
800 ◦ C–1000 ◦ C in Ar/H2 air. Changing the flow pace of the Ar/H2, the
researcher took note of the controlled layer thickness. The solid ante­
cedents give advantages similar to solid precursors in oping graphene
with heteroatoms along those lines that permit us to tune its electronic
properties with structures. Blending on the copper foils and followed by
annealing, the researchers showed this by spin coating melamine
(C3N6H6) + PMMA. N doped product is seen by subsequent graphene
and XPS demonstrates noteworthy nitrogen to be consolidated in the
graphene lattice [191]. Wrinkles appear as the quality of CVD-integrated
transferred graphene deteriorates. This method involves using photoli­
thography to conceal the basic substrate and using the remainder of the
substrate as cathodes. More than 500 nm evaporated Cu film was
required for uniform graphene formation to be reliable. Scaling up the
fabrication of CVD blended graphene films on copper and nickel foils to
wafer size has been accomplished. They’ve been mounted on
self-supporting substrates. Furthermore, as transparent leading films,
these can be used in flexible devices as well as strain sensors [192]. As a
result, graphene production on polycrystalline metal by CVD is another
promising technique for use in hardware and other applications.
3.7. Substrate induced band gap opening
This was the major approach used in graphene to estimate band gaps
provisionally. STS/STM reports of bandgap development on epitaxial h-
BN appeared in 2002, well before the primary reporting of graphene
isolation on a protective platform. Ni (111) was coated with graphene
and an exponential single layer of h-BN. The graphene/h-BN/Ni (111)
framework revealed a 0.5 eV bandgap in STS calculations [193], with a
substrate-induced gap opening. Hypothetical research on h-BN
substrate-induced graphene bandgap opening has also been carried out.
A bandgap of 53 meV may be formed in graphene on mass h-BN, ac­
cording to DFT calculations. Band structure of epitaxial graphene has
been additionally revealed on copper by the examination. It was
discovered that in graphene near-zero bandgap opened up on copper
[194]. Another current hypothetical study found that graphene on
oxygen-ended SiO2 surfaces develops a bandgap of roughly 0.52 eV, but
graphene on OH-ended SiO2 surfaces, i.e. hydrogenated, retains its
semimetal property, resulting in no covalent interaction between gra­
phene and oxygen. Particularly recently, a report on bandgap expansion
in epitaxial graphene on SiC due to substrate contact has piqued interest
7
Results in Engineering 15 (2022) 100474
due to the viability of the development technique. A schematic chart for
the equivalent is designated in Fig. 4(a). Regardless, epitaxial graphene
on SiC contains electron-doped and the Fermi level is located above the
gap. To make graphene a suitable semiconductor along these lines, it
must be gap doped or the Fermi level must be shifted in the center of the
hole by providing entryway voltage [195].
3.8. Chemical substitution doping
Among the most notable doping strategies replacement doping might
be the most notable doping as in doping conventional semiconductors, it
is the essential utilized technique. Carbon can be substituted by nitro­
gen, boron, or both in a graphitic carbon lattice to provide both n and p
doping [196]. While there has been a lot of hypothetical work on the
substitutional doping of graphene, there haven’t been many reports on
trial works confirming the hypothetical outcomes. Doping graphene
with nitrogen can turn it into a p-type semiconductor. To demonstrate
this, a significant amount of hypothetical work has been undertaken. It
has been hypothesized that N doping in ZGNRs favors the ribbon edge
energetically. Furthermore, two dopant iotas want to keep their distance
from one another. In an ongoing report that has piqued interest, nitrogen
doping has been provisionally achieved using CVD by combining
ammonia with methane as the antecedent gas on the substrate with a
thin copper film. It was possible to achieve maximum nitrogen doping of
8.9%. It also enhanced the overall exchanging percentage in the
generated FETs. In any case, doping-induced flaws resulted in a signif­
icant reduction in carrier mobility [173]. Fig. 4(b) is a diagram illus­
trating the doping point and band structure. The arc concept has also
been used to account for the amalgamation of doped graphene. DC arc
discharge and graphite terminals in an ammonia environment, large
volumes of N doped graphene have been produced. Substitutional ni­
trogen doping occurs when the nitrogen concentration is less than 1 wt
%, according to XPS estimates. The nitrogen content of nitrogen-doped
graphene has also been determined using XPS and EELS in a hydrogen+
(pyridine or alkali) environment. Similarly, substitutional boron doping
in the graphitic carbon lattice can be used in order to achieve p doping in
graphene. There have already been a significant number of potential
studies on boron-doped graphenes. The existence of substitutional boron
in the graphitic lattice increases the oxidation resistance of the graphitic
carbon test by altering the thickness conveyance of high energy elec­
trons, according to one of the most conceivable research along this
route. The inclusion of substitutional boron in the graphitic lattice in­
creases the oxidation resistance of the graphitic carbon check by
adjusting the thick movement of strong imperativeness electrons, cor­
responding to one of the most speculative studies on this topic [197]. In
any case, recent research has focused on the electrical and structural
properties of boron-doped graphenes and nanoribbons. Boron doping
causes metallic zig-zag nanoribbons to transform into semiconductors.
In addition, the substitutionally doped boron iotas prefer the edge sites
energetically in the same way that N doped boron iotas behave. GNRs
doped with substitutional boron can also operate as spin filters. Another
study found that boron edge doped zig zag GNRs exhibit half metallicity
beyond a specified basic electric field, indicating that they could be used
in upcoming spintronic devices [198]. Sending and receiving chains of 7
boron iota groups (B7) fitted into the structure of substitutionally doped
semiconducting easy chair GNRs, according to a hypothetical inquiry. A
continuing hypothetical inquiry into enormous areas of doped graphene
demonstrates that, even at doping rates as high as 4%, the transport
properties of huge zone graphene are not significantly altered. It also
claims that for high doping quality, base quantum blockage effects are
found in any case and that bearer mobilities become increasingly
doping. In boron doping, gaps are thought to be more susceptible to
localization marvels than electrons. Boron-doped graphenes have also
been merged by arc discharge, either in a hydrogen + B2H6 (diborane)
environment or using boron-filled graphite anodes, much like the
nitrogen-doped graphenes. STM and Raman’s measurements confirmed
R. Nandee et al.
Fig. 7. Variations of the electronic band structures of monolayer graphene near the K point with increasing sodium coverage. (a) Atomic structure and first Brillouine
zone of monolayer graphene. (b) ARPES intensity map of the pristine monolayer graphene along the ky direction. (c–g) ARPES intensity maps of the sodium-adsorbed
monolayer graphene along the ky direction. In (b–g), the dispersions (white lines) were extracted from the EDC peak positions and the blue lines are EDCs obtained at
the K point. (h) MDCs at the EF of the ARPES maps in (b–g) [206].
that boron substitutional doping increases the number of defects and
disorders in graphene layers [199]. In any event, there haven’t been
many instances of substitutional doping, and uniform doping over a
large area of graphene hasn’t been performed satisfactorily until now.
Furthermore, the bearer portability and conductivity estimates of sub­
stitutionally doped graphene are substantially inferior to those of im­
maculate graphene. Regardless, it is one of the most promising
approaches for opening a bandgap in a large zone of unattached
graphene.
4. Hybrids
Doping graphitic carbon cross-section with both boron and nitrogen
at the same time framing BCN solid configurations in hexagonal grid and
production of single-layer BCN semiconductors and Bx Cy Nz nanotubes
have been studied for a long time. Several preliminary studies show the
effective synthesis of BCN materials [200–203]. CVD has also been used
to combine BCN films with C, B, and N precursors. Regardless, the
thickness of these films has been requested in the range of nanometers to
microns. Furthermore, the translucency of these films was weak. Each of
these papers describes atomic hybrids of B, C, and N with semi­
conducting electrical characteristics. However, when the B–C–N stage
outline is examined, it is observed that boron and nitrogen tend to
isolate and produce h-BN, which is also energetically favorable [204].
8
Results in Engineering 15 (2022) 100474
The formation of graphene-h-BN combinations is becoming more
possible. Indeed, this framework has been hypothetically investigated
and, more recently, experimentally synthesized. Although laser vapor­
ization has previously been used to include hybrid C–BN nanotubes with
BN regions, there has been no report on their electrical characteristics.
Bandgap opening in such hybrid nanotubes has been discovered through
theoretical research on a comparable framework. It was also stated that
the N-ended BN spaces were the most consistent enthusiastically. A
theoretical investigation of h-BN/GNR/h-BN sandwiched hybrid nano­
ribbon architectures has also recently been described. This structure is
essentially stable, and ZGNRs sandwiched between h-BNs act as half
metals, with potential uses in spintronics. These films were also com­
bined over a range of C and BN concentrations. A little band hole
opening was detected, as well as an exceptional double optical band
hole. Because these films possessed anisotropic structure, the approach
appears to be exceedingly promising for merging hybrid films with
tunable electrical and optical properties. Hypothetical calculations done
in a related article also suggest band hole opening in hybrid with BN
areas and that the band hole increases with decreases in h-BN space size
[205]. Fig. 7 illustrates this. Although this technique appears promising,
control over area size and shape has not yet been achieved, which is
required for tweaking the gap and other electrical properties.
The immediate awareness of turn energized edge states for zigzag
edge topologies, such as ZGNRs, was not possible until recently due to
R. Nandee et al. Results in Engineering 15 (2022) 100474

Fig. 8. (a) Cutting graphene into nanoribbons with different edge topologies. Indices (m, n) are used to denote the dimensions of a graphene nanoribbon (GNR) along
the zigzag (m) and armchair direction (n), respectively. (b) Sketch of energy levels for a finite (7, 12) GNR, with ΔAC and ΔZZ indicating the bulk band gap and the
splitting of the localized states at the zigzag edges, respectively. (c) Kohn–Sham spin-orbitals of edge-localized states and energetically closest bulk states. Electrons
with different spins are localized at opposing zigzag edges [207].

Fig. 9. Schematics illustration of the procedures to produce the graphene film for surface patterning using femtosecond laser pulses. (a) Graphene oxide sheets. (b)
Reduced graphene sheets. (c) Graphene film by filtration of reduced graphene sheets. (d) A graphene microflower produced with a single laser pulse at fluence of 1.1
J/cm2. (e) Large-area surface patterning by fs laser direct writing. (f) Large-area uniform flower patterns on the surface of a graphene film. Digital image of the
pristine (left) and engineered surfaces (right, darker black) showing totally different surface wettability [225].

the limited reliability of current top-down methods Using ground which exhibited the nearby bond arrangements at small separations
polymer and cyclodehydrogenation of carefully defined forerunner (Fig. 8) and genuinely validated the regular example of 6-ZGNRs. Edge
monomers, the base up synthesis of ZGNRs with molecularly exact states were detected after 6-ZGNRs were driven with the STM point into
zigzag edges was established in 2016 [208]. Additional fundamental post-stored insulation islands of NaCl and electronically disengaged
facts were exposed with the assistance of non-contact nuclear power from the metal substrate.
microscopy (nc-AFM) imaging with a Founder tip, which exhibited the
nearby bond arrangements at small separations (Fig. 8) and genuinely
4.1. Laser shocking
confirmed the typical structure of 6-ZGNRs. Edge states were seen after
6-ZGNRs were directed with the STM tip into post-stored insulated
Researchers used a photonic technique to modulate graphene’s
islands of NaCl and electronically dissociated from the metal substrate.
bandgap structure and vibrational energy, resulting in bandgap en­
Additional fundamental facts were discovered with the assistance of
hancements of 1.7–2.1 eV and a Fermi-level spread of 0.6 eV for the first
non-contact atomic power imaging (nc-AFM) imaging with a Cross tip,
time. To acknowledge the nonuniform proximal local asymmetric

9
R. Nandee et al. Results in Engineering 15 (2022) 100474

Fig. 10. Trilayer graphene sheet resistances as a function of pressure and temperature (A) at room temperature, resistance–pressure curves of trilayer graphene (300
K). The strong black lines serve as visual guidelines. The black dotted line represents the resistance quantum, h/4e2 6.45 k, beyond which Anderson localization
causes a disordered conductor to act as an insulator at low temperatures. (B) Semimetallic–semiconducting transition R-T curves at representative pressures (C)
Resistance Arrhenius plots by which equation is fitted to the solid red lines. (Inset) The obtained activation energy E1 and its pressure dependency are depicted. The
fitting errors and critical temperature selection of these three transport mechanisms are the sources of uncertainty [251].

elastomeric tension in graphene, laser shock engraving is used to create
a strain rate (d/dt) of 106 s1 in this study shown in Fig. 9. This results in
excellent formability and rigidity of graphene [209,210]. Pressure can
be adjusted by adjusting the episode cutting speed. Memphis carbon was
screwed onto an e-bar generated SiO2 nano mold with planned mor­
phologies by laser shocking to widen its bandgap, which can still be
controlled, culminating in a designed strain profile over out The task is
adjustable with a region of 0.6 eV, which is enough for resource layer
personality in electromagnetic shielding electrical and photoelectric
equipment to acquire stimulating achievements, so according to Kelvin
probe force imaging (KPFM) mental effects of the strained monolayer.
Scanning electron microscopy and nuclear power projection were used
to study the warped surface profile. Through scanning tunneling spec­
troscopy, the electronic bandgap of single-layer inhomogeneous strain
graphene was studied. Transmission electron microscopy and nuclear
power imaging were used to characterize the altered sample selection.
Using scanning tunneling spectrometry, the electromagnetic bandgap of
single-layer stress graphene was evaluated.
By applying non-symmetric polycarbonate stresses to nanomaterials,
laser shock created large nanocrystalline digital bandgaps even as other
graphene properties could be tuned, such as the graphene work
function.
Materials science, digital, and photonic applications are poised to
benefit greatly from non-homogeneous straining by beam shock
[226–229]. The experimental arrangement is depicted in Fig. 9. Gra­
phene is sandwiched between an aluminum film and a-Si/SiO2 mold.
The aluminum film is smashed by the laser shock, causing a large strain
to be transferred to the graphene layer. By varying the laser power, a
pressure shock of several tens of gigapascals can be produced, resulting
in 3D inhomogeneous strain in monolayer graphene: an inset shows a
small-scale MD simulation of stretched monolayer graphene produced
by laser shock. Fig. 1(b) shows the evolution of nano-shaped graphene.
In the additional information depicts an animation of the simulation
process for producing strained monolayer graphene. On SiO2, nano­
trenches with controlled dimensions (width and depth) were created by
electron beam lithography (EBL), which was then used to form a mold
for laser shock nanoimprinting. Fig. 9 show typical molds with varying
trench widths on a single substrate. Nanotech molds are shown in detail
in Fig. 9. In Fig. 9, nano strained laser shock nanoimprinted graphene
has the same width of 400 nm and depth of 100 nm corresponding to the
mold shape, demonstrating that the smooth curvature of the atomic
structure can be precisely defined by the mold dimension and laser
shock pressure. Additionally, we measured the Raman spectra of gra­
phene after laser shock at eight different nanotrenches and another
location between nanotrenches. Fig. 9 shows their Raman spectra
mapped. Our experiments deliver the laser shock directly to an
aluminum foil, causing large strains to be transferred to graphene,
allowing laser-induced defects in graphene to be ignored. Additionally,
Raman peak shifts may be reduced by using high-quality graphene and a
clean transfer process. Thus, the Raman peak shifts can be attributed to
graphene’s high strain. In response to laser shocking, the 2D peak (2680
cm-1) and G peak (1600 cm-1) both show an obvious red shift from
points b-h, indicating that strain is greatest at the trench edge and then
decreases from the trench edge to the trench center. In addition, the
intensity ratio between D peak (1350 cm-1) and G peak (ID/IG) is
calculated to analyze the crystal quality of graphene after laser treat­
ment. These ratios are less than 0.7, with the greatest ratio at the trench
edge with the greatest strain. The ratios decrease from the edge toward
the center, with a minimum value close to that of unstrained chemical
vapor deposition (CVD) monolayer graphene, consistent with the strain
distribution on graphene after laser shock. To evaluate laser shock nano
training of graphene on e-beam fabricated nanotrench-shaped nano­
molds for electronic bandgap engineering, scanning tunneling spec­
troscopy and other analytical techniques were used. As a consequence of
the imprinting of nanoscale ultrahigh strain rates during laser stunning,
we observe strain tunable bandgap formation in graphene, with
bandgap values ranging from 1.7 to 2.1 eV. Graphene has never
demonstrated such a high level of bandgap development with no
extrinsic effects except for graphene itself, and this is the first of its kind.
As a result of such a tunable bandgap formation in graphene, it is
possible to convert semimetallic graphene into semiconducting gra­
phene with a wide frequency band.
5. Other advanced materials
Good numbers of methods are available to modify the electronic
structure of graphene for substantial bandgap. Doping is a good
approach that helps to tune the bandgap in graphene [230]. Inter­
changing the electrons between graphene surface transfer doping can be
achieved by surface transfer doping which does not interrupt the gra­
phene structure and is reversible [231]. Replacing the carbon atom with
a foreign atom in the graphene lattice, substitutional doping is achieved

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R. Nandee et al. Results in Engineering 15 (2022) 100474

Fig. 11. MLG reversible hydrogenation under electric-field control a, Electric measurement arrangement and schematic of an HIE-gated graphene device b, The
hydrogenation of the graphene lattice (blue) by H+ ions is depicted (red). c, Three cycles of IDS measurements in device M1 as a function of gate voltage VG at room
temperature (25 ◦ C), demonstrating a very reproducible conductor–insulator transition in the MLG. VG’s sweep directions are indicated by black arrows. The applied
VDS is set to 5 mV. d, MLG Raman spectra in Device M2 with various VG values. The solid dot and circled number with the same color in c represent the equivalent
IDS of the labelled VG. The relationship between IDS and Raman spectra at various VG values is largely repeatable across devices. The intensity of VG = 2.0 V is
divided by four to clearly depict all Raman spectra [252].

that has the capability to charge the infusion. Directing a beam of
electrons and using scanning transmission electron microscopy, the gap
defect is formed [232]. Chemical reduction is another approach that is
very simple and can be performed at low temperatures using different
reducing agents [233]. This approach leads to a substantial opening of
the bandgap in graphene. There are some other approaches as well
which are good for bandgap tuning such as cutting graphene into
nanoribbons [234] or nanomeshes [235], applying a perpendicular
magnetic field to bilayer graphene [236], configuring (ordering of im­
purity atoms [237–239], applying different strains such as uniaxial
tensile [240–245] and shear [246,247] deformations or their combina­
tion [248,249] and Straintronics [250].
6. Future challenges and prospect
electrochemical hydrogenation in an organic liquid electrolyte con­
taining dissociative hydrogen ions may be used to control the
conductor-to-insulator transitions in microscale graphene using an
electric field. At normal temperature, completely hydrogenated gra­
phene has a lower sheet resistance limit of 200 G sq-1, allowing gra­
phene field-effect transistors to have on/off current ratios of 108. With
up to 1 million switching cycles, the gadgets also have a long life span.
Bilayer graphene exhibits similar insulating properties; however, tri­
layer graphene following hydrogenation remains extremely conductive.
The transition from sp2 to sp3 hybridization is accompanied by changes
in the graphene lattice. The concept is illustrated in Fig. 11.
The challenges of formation of sizeable band gap in graphene are also
studied experimental and theoretical studies [254–256], but the desired
level is yet to be less understood.

6.1. Future prospect and challenges of sizable bandgap from trilayer 6.2Future prospect and challenges of low contact resistance metal
graphene semiconductor interface

Graphene is a miracle of materials research due to its extraordinary
physical properties. However, graphene’s gapless nature precludes it
from becoming a serious candidate for post-silicon electronics. As a
result, opening a large bandgap in graphene is greatly desired. On
nanomaterials with only a few layers, Researchers [251] devised a micro
wiring technique for high-pressure electrical monitoring. They showed
that in compressed Bernal-stacked trilayer graphene, an inherent
bandgap of 2.5 eV may be achieved using in situ electrical and absor­
bance experiments (Fig. 10). The achievement of a broad bandgap in
compressed graphene encourages research into the practical application
of carbon-based electronics.
A hydrogenation reaction, which transforms graphene into insu­
lating graphane with sp3 bonding, is one method for introducing an
energy gap. The research [252,253] showed that reversible
Researchers have developed a low contact resistance metal-
semiconductor interface computationally using 2D monolayers for
next-generation transistors, which could improve device performance.
Graphene, a flat monolayer of carbon atoms of graphene organized
in a 2D honeycomb lattice is of research interest. But the lack of resis­
tance in pristine graphene is a significant drawback to its use in elec­
tronics and switching devices. It is unable to manage the current flowing
through it or to switch from an on to an off state. As a result, 2D semi­
conductors have evolved throughout time to overcome the constraints of
graphene. New 2D semiconducting monolayers (MgX X = S, Se, Te) with
high charge carrier mobility have been proposed by researchers at the
Indian Institute of Nanoscience and Technology (INST), an autonomous
institute of the Department of Science and Technology (DST).
The proposed monolayers are unique in that they integrate

11
R. Nandee et al. Results in Engineering 15 (2022) 100474

Fig. 12. For different configurations, contour maps show the charge-density differential between tBLG and superposition of two individual graphene layers [261].

Fig. 13. Relationship between induced energy band gap and applied electric field strength [272].

12
R. Nandee et al. Results in Engineering 15 (2022) 100474

Table 1 superposition of two separate graphene layers with charges evenly

Energy bandgape in different process. distributed at all sites for different configurations (see Fig. 13)(see
Reference Dopant atoms No. of atoms Band gap Table 1).
(eV) The electronic characteristics of single and bilayer graphene were
[211] B 1, 2, 3 0.14, 0.2, 0.4 studied using the Hamiltonian tight-binding model. Under the influence
N 1, 2, 3 0.14, 0.2, 0.4 of an electric field, the energy band gap of bilayer graphene can be
[212] N 1, 2 0.15, 0.2 adjusted from 0 to 0.29 eV. The study [262] showed that the charge
[213] B 1 0.14 distribution in the inter and intra-graphene layer determines the energy
[214] BN co-doped impurity Band 5B/5 N 0.35
gap
bandgap structure, based on energy bandgap analysis from Hamiltonian
[215] Be 0.25 tight-binding simulations. Under DC and low amplitude electric field
Mg 0.5 potential for optical excitation, the bandgap of bilayer graphene can be
Ca 0.4 controlled using the applicable technique. The changeable bandgap of
Ba 0.45
bilayer graphene under the applied electric field is shown in Fig. 9. The
Sr 0.11
[214] H 0.45 induced energy bandgap grows linearly in proportion to the applied
[216] H, Au 1 electric field strength. There are similar other studies that are available
[117] SiC 0.23 in the literature but most of them are on a theoretical level [263–265].
[218] N Content 4% Atom 0.3 Bandgap formation in graphene nanoribbons and quantum dots
[219] BN Content 35% 1.62
Atom
[266–271] are considered promising technologies for ensuring the ver­
BN Content 16% 1.51 satile applications of graphene. But these studies are also on the theo­
Atom retical level and their implications in the practical field are even now
[220] Si 0.13 to 0.25 considered a challenging issue.
[221] SiO2 0.35
The band gap formation of 2D materials are also be correlated to
[222] Cu 0.18
[217] Ag 0.32 immune response, crude oil recovery from sand, field reduction simu­
[223] Cu 0.25 lation based on covered conductors, packing density in future
[224] Na–Ir 0.74 [273–276].
The synthesis processes, characterization process, graphene nano­
particle trends and some other properties [277–280] are another chal­
flexibility, spintronic, and piezoelectric capabilities in a synergistic
lenging issues to confirm the better quality of graphene band gap.
manner, making them desirable for self-powered nanoelectronics de­
vices in the future.
6.4. Future prospect and challenges of micromechanism
The researchers [257] investigated reduced contact resistance be­
tween semimetal graphene and MgX in a study published in Phys. Rev.
The consideration of micromechanism to improve the properties of
B. They discovered complete non-resistive contact at the graphene-MgS
graphene for band gap opening has promising future. In recent years,
interface, a rare and highly desired state for charge transport through
graphene foams (GrFs) have gotten a lot of attention from scientists and
the channel. Vertical strain and an electric field are used to modulate
engineers [281]. Its future applications require good elasticity. How­
electrical contact characteristics. This research looks at
ever, the mechanism and basic properties of GrF elasticity are yet un­
non-invasive/non-destructive bandgap opening, stacking-dependent
known. The flake bending, rather than the stretching, dominates the
contact characteristics, and charge carrier concentration tunability in
deformation of GrFs, which is independent of the loading type, size,
pure graphene. This research can be applied to electrical and spintronic
shape, or thickness of flakes, as well as the density or stiffness of
devices based on graphene. The proposed low contact resistance
crosslinks. Different modes of bond breaking cause significant asym­
metal-semiconductor interface computational concept is depicted in
metry in elasticity under tension and compression. Furthermore, the
Fig. 11. Similar computational works have been done for other materials
larger flakes and more crosslinks are two crucial elements that
for confirming the effectiveness of graphene bandgap in low content
contribute to GrFs’ flexibility.
resistance devices [258–260].
In recent years, nanoparticle-contained graphene foams (NP-GrFs)
The computational findings are intended to inspire the experimental
have received a lot of attention and have been employed in a lot of useful
work to create futuristic electronic devices with the needed function­
applications. However, the mechanical property of such a novel com­
ality, such as piezofield effect transistors.
posite material, as well as its micro-mechanics, is still unknown. The
mechanical responses of NP-GrFs under uniaxial tension, as well as the
6.3. Future prospect and challenges of tunable band gap in graphene size and volume fraction effects of nanoparticles, are thoroughly studied
in this work using a coarse-grained NP-GrFs model [282]. The initial
Twisted bilayer graphene with even parity under sublattice exchange modulus and tensile strength of NPs are shown to be dependent on their
has modest gap at large comparable angles. It has been shown how to size and volume percentage, both of which can rise by almost an order of
turn this small gap into a large one. This study began by using density magnitude. Furthermore, the strain hardening phenomena happens as
functional theory calculations to gain a thorough grasp of the physical the volume fraction of nanoparticles increases. There are two main
origins of gap opening. The effective interlayer hopping, intralayer improving mechanisms discovered. The enhanced adhesion between
charge-density-wave, or interlayer charge imbalance favors a gap. Then, neighboring sheets caused by NPs and the homogenized stress caused by
based on tight-binding calculations, a periodic transverse inhomoge­ NP extrusion are two examples. The current findings should be valuable
neous pressure, which can adjust interlayer hoppings in specific regions not only in understanding the microstructure-dependent mechanical
of the more supercells, might open a gap of over 100 meV, which is properties of NP-GrFs, but also in the development of novel functional
supported by first-principles calculations. The work concentrates on the materials and devices based on GrFs.
theoretical guidance for efforts involving twisted bilayer graphene that Due to its exceptional multi-functional features, particularly its
aim to bridge a wide gap. In reality, gap opening is aided by intralayer dissipation capability, graphene foam (GrF) is a new type of multi-
CDW or interlayer charge imbalance. To acquire a bigger gap in tBLG, it porous material with various potential applications. However, the
is necessary to understand the impact of interlayer hoppings, intralayer dissipative process as well as several experimental observations are yet
CDW, and interlayer charge imbalance [261]. Fig. 12, presents contour unknown [283]. First, the typical stress-strain relationships obtained in
maps of the charge-density difference between tBLG and the studies under large-strain loading-unloading and small-strain cyclic load

13
R. Nandee et al.
Fig. 14. Present and future applications of graphene and its global economic impact (partly of the figure adapted from ref. [167]).
are replicated. Microstructure study found three key dissipative mech­
anisms at the size of flakes: rippling, sliding, and hitting. The impacts of
cycle number, strain magnitude, and loading rate on dissipation are
examined in greater depth. The substantially larger dissipation in the
initial loading cycle is discovered to be mostly owing to drastic flake
rearrangements, which reduce to a lesser one in future cycles. Further­
more, due to the flake stacking patterns, the dissipation increases
approximately linearly with the strain magnitude in the first cycle, but
with a lower slope in future cycles. The dissipation will increase as the
loading rate increases for a particular strain magnitude. These findings
add to our knowledge of GrFs’ dissipative mechanism and should aid in
the creation of new multifunctional graphene-based composites.
Similar other studies [284–287] are carrying out to understand the
limitation of the micromechanism in relation to the different operating
and processing parameters for the improvement of graphene properties,
hence the sizeable and tunable bandgap formation.
7. Conclusions
The bandgap of semiconductor graphene is virtually zero, which is a
unique property. At the beginning of the valence band, graphene’s
charge carrier velocity remains constant, unlike some other materials. In
recent years, interest in it has increased due to its unique semi-metallic
properties, highly conductive, no bandgap, and electron’s relativistic
nature. This study critically evaluated the recent advancement
regarding bandgap formation of graphene, especially in the area of
doping, synthesis, mechanical exfoliation, substrate-induced band gap
opening hybrid, and laser shocking. The wonder material, graphene, has
applications in integrated circuit design, transistors, flexible electronics,
and photovoltaics, among others. Graphene may become more
appealing than silicon-based electronics after complete development, on
a large scale, of films with desired electrical properties. This would allow
future electric devices to be fast, chemically stable, environmentally
friendly, and functional. So, there is a great need for research to increase
graphene’s bandgap and improve its functionality to meet the demands
of the modern world. But even though there are lots of challenges in the
applications of graphene semiconductors. The sizeable bandgap, low
contact resistance, and tunable properties are even now in the
14
Results in Engineering 15 (2022) 100474
theoretical stage. The researchers have a lot of opportunities to use the
concept of theoretical results for the experimentation for a better un­
derstanding and its wide range of electronics applications. Considering
the present and future applications of graphene and its global economic
impact on the industry (Fig. 14), this article can be used as a reliable
source and state of art for the researchers.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
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